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Implantation of Ni nano domains in refractory metal oxide support by means of sol-gel encapsulation—an effective solution to coke formation in the partial oxidation of natural gas

a technology of refractory metal oxide and nano-domains, which is applied in the direction of metal/metal-oxide/metal-hydroxide catalysts, physical/chemical process catalysts, bulk chemical production, etc., can solve the problem of deactivation of industrial reforming of light hydrocarbon gases, and achieve high methane conversion and immunity to coking

Inactive Publication Date: 2014-02-25
NAT UNIV OF SINGAPORE
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  • Summary
  • Abstract
  • Description
  • Claims
  • Application Information

AI Technical Summary

Benefits of technology

[0009]In still another aspect, this invention features a method of producing carbon monoxide and hydrogen by partial oxidation of a C1-C5 hydrocarbon. In this method, a gaseous stream containing a C1-C5 hydrocarbon and oxygen gas is fed into a reactor, in which the above-described metal-oxide supported nickel catalyst is placed to produce carbon monoxide and hydrogen at 700-900° C. The metal-oxide supported nickel catalyst used in this method, as mentioned above, contains catalytic sites that can be nano-nickel(0) domains or nano-nickel(0)-A(0) alloy domains and have a particular interface with the matrix. This interface can effectively prevent the Ni domains from merging at a typical catalytic dry reforming temperature (800-900° C.). As a result, the catalyst becomes highly immune to coking. For example, it can retain a high methane conversion (XCH4>90%) and syngas selectivity (SCO>85%) over a long run (e.g., 6 hours) of partial oxidation of methane.

Problems solved by technology

Currently, the obstacle to the industrial reforming of light hydrocarbon gases is still deactivation of metal oxide-supported Ni(0) catalyst due to deposition of carbon on Ni(0) catalytic sites.

Method used

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Examples

Experimental program
Comparison scheme
Effect test

example 1

Preparation of Al2O3-Supported Ni Catalyst

[0025]15.0 g Ni(NO3)2.6H2O and 5.0 g n-hexadecyl trimethylammonium bromide (CTAB) were dissolved in 100 ml water at 65° C. with stirring, and then after the solution was cooled down to room temperature 10 ml tetramethylammonium hydroxide (TMAH, 1.0 M aqueous solution) was added into it with immediate blending. A stable (NixOy)(OH)2(x−y) colloidal suspension was formed after the above mixture was stirred for about 1 hour. This was followed by the introduction of 60 g aluminum isopropoxide into the resulting (NixOy)(OH)2(x−y) colloidal suspension at room temperature, and the suspension formed was ball-milled using ceramic media for 72 hours, which led to a homogeneous sol dispersion. This sol-dispersion was thickened at 80° C. to form a solid gel, and the solid gel was finally subjected to calcination at 600° C. for 4 hours to generate an Al2O3-supported Ni catalyst with 22 wt % nickel loading.

example 2

Preparation of SiO2-Supported Ni Catalyst

[0026]15.0 g Ni(NO3)2.6H2O and 5.0 g CTAB were dissolved in 100 ml water at 65° C. with stirring, and after the solution was cooled down to room temperature 10 ml TMAH (1.0M aqueous solution) was added into it with immediate blending. A stable (NixOy(OH)2(x−y) colloidal suspension was formed after the above mixture was stirred for about 1 hour. This was followed by the introduction of 60 ml tetraethyl orthosilicate (TEOS) into the resulting (NixOy(OH)2(x−y) colloidal suspension at room temperature. The mixture was homogenized by stirring overnight at room temperature and then the stirring was continued at 65° C. for additional 24 h to allow complete hydrolysis of TEOS to form a sol suspension. This sol-dispersion was converted to a solid gel after being thickened at 80° C., and the solid gel was finally subjected to calcination at 600° C. for 4 hours to generate a SiO2-supported Ni catalyst with 18 wt % nickel loading.

example 3

Preparation of CaO-Supported Ni Catalyst

[0027]15.0 g Ni(NO3)2.H2O and 5.0 g CTAB were dissolved in 100 ml water at 65° C. with stirring, and then after the solution was cooled down to room temperature 10 ml TMAH (1.0 M aqueous solution) was added into it with immediate blending. A stable (NixOy)(OH)2(x−y) colloidal suspension was formed after the above mixture was stirred for about 1 hour. This was followed by addition of 12 g CaO into the resulting (NixOy)(OH)2(x−y) colloidal suspension at room temperature, and the suspension was ball-milled using ceramic for 72 hours. In this process, the surface of CaO becomes a hydrogel layer comprising Ca(OH)2 species in the basic medium. Therefore, (NixOy)(OH)2(x−y) sol particles can effectively enter in this hydrogel layer. The suspension was thickened at 80° C. to form a solid gel and the solid gel was finally subjected to calcination at 600° C. for 4 hours to generate a CaO-supported Ni catalyst with 22 wt % nickel loading.

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Abstract

A metal oxide-supported nickel catalyst includes a matrix containing a metal oxide and catalytic sites distributed throughout the matrix and having an intricate interface with the matrix, in which the catalytic sites are selected from the group consisting of nano-nickel(0) domains and nano-nickel(0)-A(0) alloy domains. Also disclosed are a method for preparing this catalyst and a method for using it to produce carbon monoxide and hydrogen by partial oxidation of a C1-C5 hydrocarbon.

Description

CROSS-REFERENCE TO RELATED APPLICATIONS[0001]This application is the National Stage of International Application No. PCT / SG2011 / 000090, filed on Mar. 8, 2011, which claims the benefit of the priority date of U.S. Provisional Application No. 61 / 311,657, filed on Mar. 8, 2010. The contents of these applications are hereby incorporated by reference in its entirety.BACKGROUND OF THE INVENTION[0002]Catalytic partial oxidation (or dry reforming) of methane (POM), other light alkane compounds existing in natural gas (e.g., C2-C5 alkanes), and alcohols producing synthesis gas (CO+2H2) can be integrated as an anodic reaction (CH4+O2−→CO+2H2+2e−) with the electrochemical separation of air (½O2+2e−→O2−), a cathodic reaction, to form a catalytic membrane reactor. This combination has paramount commercial value in terms of saving energy and production of H2, N2, and a series of useful chemical intermediates. Currently, the obstacle to the industrial reforming of light hydrocarbon gases is still ...

Claims

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Application Information

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Patent Type & Authority Patents(United States)
IPC IPC(8): B01J23/00
CPCB01J37/18B01J37/033B01J23/892B01J23/78C01B2203/1247B01J23/02C01B2203/1058B01J37/0036B01J23/755C01B2203/1241B01J37/036B01J21/04B01J37/16C01B2203/0261C01B3/26B01J21/066C01B3/40B01J21/08B01J21/06Y02P20/52
Inventor HONG, LIANGYIN, XIONG
Owner NAT UNIV OF SINGAPORE
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